Exploring Single‐Phase Asymmetric Multiple‐Quantum‐Well Architectures in Chiral Hybrid Perovskites via Kinetically Controlled Self‐Assembly

Abstract

AbstractChiral hybrid perovskites (CHPs) with inherent chirality, dimensional tunability, and excellent semiconducting features are proved to be an ideal platform to study spin and helicity‐related physical phenomenon. However, due to their intrinsic thermodynamic unfavorability, there are many CHPs with exotic structures, such as superlattice‐type 2D heterostructures, which are covered by their transient lifespan caused by phase instability during the crystallization process. This limitation hinders the attempt to further explore and understand the chiral structure‐function relationship. Here, CHPs (R/SCPEA)2PbI4·(R/SCPEA)2FAPb2I7 (R/S1‐2, R/S‐CPEA = (R/S)‐1‐(4‐chlorophenyl)ethylammonium FA = formidinum) is obtained with asymmetric multiple‐quantum‐well architectures through kinetically‐controlled self‐assembly. Structural analysis identified the unique natural monolayer‐bilayer recurring heterostructures of 1–2 with sub‐nanometer accuracy and potentially non‐degenerate chiral environment. Such novel structures in 1–2 provide them fascinating multiple absorption‐emission features. Meanwhile, the chirality of 1–2 is confirmed by vibrational circular dichroism and angle‐dependent photocurrent measurement, provoking its potential in chiral optoelectronic devices. The work extends the understanding of CHP growth and will stimulate further exploration and synthesis of extraordinary chiral heterostructures, which may pave the way for the development of chiral optoelectronics and spintronics.